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Exfoliated TiNbO5 nanosheets were obtained by delaminating a layered compound KTiNbO5.Employing a layer-by-layer electrostatic deposition technology, the exfoliated nanosheets were deposited into a multilayer composite film with polyethylenimine as the linker, confirmed by UV-vis absorption spectra and X-ray diffraction.The polymer-free TiNbO5 nanosheet multilayer film was achieved through the subsequent ultraviolet light exposure.